|Publication number||US6852555 B1|
|Application number||US 09/720,329|
|Publication date||Feb 8, 2005|
|Filing date||Apr 14, 2000|
|Priority date||Apr 22, 1999|
|Also published as||CA2370852A1, CN1201396C, CN1348606A, EP1194957A1, WO2000065653A1, WO2000065653A9|
|Publication number||09720329, 720329, PCT/2000/127, PCT/NO/0/000127, PCT/NO/0/00127, PCT/NO/2000/000127, PCT/NO/2000/00127, PCT/NO0/000127, PCT/NO0/00127, PCT/NO0000127, PCT/NO000127, PCT/NO2000/000127, PCT/NO2000/00127, PCT/NO2000000127, PCT/NO200000127, US 6852555 B1, US 6852555B1, US-B1-6852555, US6852555 B1, US6852555B1|
|Inventors||Lucimara Stolz Roman, Olle Inganäs, Olle Hagel, Johan Carlsson, Göran Gustafsson, Magnus Berggren|
|Original Assignee||Thin Film Electronics Asa|
|Export Citation||BiBTeX, EndNote, RefMan|
|Patent Citations (17), Non-Patent Citations (11), Referenced by (46), Classifications (18), Legal Events (4)|
|External Links: USPTO, USPTO Assignment, Espacenet|
This application is the national phase under 35 U.S.C. § 371 of PCT International Application No. PCT/NO00/00127 which has an International filing date of Apr. 14, 2000, which designated the United States of America.
The present invention concerns a method for the fabrication of an organic thin-film semiconducting device, wherein the semiconducting device, comprises an electrode arrangement with electrodes contacting the semiconducting organic material.
The invention also concerns applications of the method according to the invention.
Particularly the invention concerns the modification of the injection properties of electrodes in an electrode arrangement for a semiconductor component manufactured with organic semiconducting material.
A paper by M. Granström et al., “Laminated fabrication of polymeric photovoltaic diodes”, Nature, Vol. 395, pp. 257-260, discloses a photovoltaic diode with a double layer of semiconducting polymers. Photoexcited electron transfer between donor and acceptor molecular semiconductors provides a method of efficient charge generation after photoabsorption and can be exploited in photovoltaic diodes. But efficient charge separation and transport to the collector electrodes are problematic, because the absorbed photons must be close to the donor-acceptor heterojunction, while at the same time good connectivity of the donor and acceptor materials in the respective electrodes is required. Mixtures of acceptor and donor semiconducting polymers can provide phase-separated structures, which to some extent meet this requirement, and provide high photoconductive efficiencies. To this endGranström et al. disclose two-layer polymer diodes where the acceptor material is a fluorescent cyano derivative of poly(p-phenylene vinylene) (MEH-CN-PPV) doped with a small amount of a derivative of polythiophene (POPT). The acceptor layer is contacted by an electrode and covered by a glass substrate. The acceptor layer is laminated together with a donor layer of POPT doped with a small amount of MEH-CN-PPV which is spin-coated on either indium tin oxide (ITO) substrates or glass coated with polyethylene dioxide thiophene (doped with polystyrene sulphonic acid) (PEDOT-PSS). To ensure a low contact resistance, a thin layer of gold was thermally evaporated on the glass substrate before the PEDOT material was spin-coated thereon. SinceGranström et al. describe a photovoltaic diode, it is evident that they are not concerned with obtaining a high rectification ratio,as is desirable with switching diodes, nor is a difference in the work function values of the cathode and the anode an issue, although the materials envisaged for the anode, (ITO, PEDOT and gold) all have a high work function value, ranging from 4.8 for ITO to well above 5 eV for PEDOT and gold, with the work function values of the latter two being almost the same.
However, it has been found that particularly noble metals such as gold and platinum result in a poor quality of a conducting polymer thin film deposited and very often the polymer film has pin holes which are not acceptable when the films are arranged in a sandwiched geometry. Moreover gold is a costly material, although Granström et al. selected gold because of its high work function value matching that of PEDOT-PSS.
In switching semiconductor devices with diode structures a high rectification ratio at of the latter is desirable. It is also desired that the contact surface between an electrode and a semiconducting polymer provides efficient charge injection, but this latter feature is not of concern for collector electrodes, that are the anodes, in a photovoltaic device based on organic semiconducting materials.
It is known that the contact surface between a conducting and a semiconducting polymer has superior properties with respect to injection of charge. For example a conducting polymer based on poly(3,4-ethylenedioxythiophene) (PEDOT) possesses a very high work function which makes it suitable as anode in semiconductor components based on organic semiconductors, but the high resistivity of PEDOT limits the performance of components because of a very high series resistance. This is particularly unfortunate when the electrodes are patterned with line widths of the order of 1 μm. However, it is believed that such components shall be crucial to realizing high density memory cells for use in memory modules based on polymers as the memory material, provided that it is possible to achieve the desired high data read-out speed. This shall, however depend on the availability of highly conducting electrodes for the memory cells which can be manufactured with microfabrication methods.
The object of the present invention is therefore to provide a method for the manufacturing of an electrode for use in organic semiconductor components, and such that the electrode combines superior charge injection properties with a high conductivity. Furthermore it is an object of the invention to provide a method which permits the manufacturing of an electrode of this kind with patterned line widths in the order of 1 μm. Finally it is also an object of the present invention to provide a method for manufacturing of electrodes which can be used in organic thin-film diodes, with high rectification ratio, or in electrode arrangements in organic thin-film transistors.
The above-mentioned objects and advantages are achieved by a method according to the invention which is characterized by depositing a first layer of a conducting or semiconducting material or combination of a conducting and a semiconducting material in the form of a patterned or non-patterned layer on an insulating substrate, such that at least a portion of the substrate is covered by the first layer, modifying the work function of the conducting and/or semiconducting material of the first layer by depositing a second layer of a conducting polymer with a work function higher than that of the material in the first layer such that the layer of the conducting polymer mainly covers the first layer or is conformal with the latter, whereby the combination of the first layer and the second layer constitutes the anode of the electrode arrangement and the work function of the anode becomes substantially equal to that of the conducting polymer, depositing a third layer of a semiconducting organic material on the top of the anode, and optionally and in case only a portion of the substrate is covered by the anode, also above at least some of the portion of the substrate not covered by the anode, and depositing a patterned or non-patterned fourth layer of a metal on the top of the third layer, whereby the fourth layer constitutes the cathode of the electrode arrangement.
It is according to the invention advantageous when the conducting material of the first layer is a metal and preferably the metal is selected among calcium, manganese, aluminium, nickel, copper or silver. It is also preferred that the semiconducting material of the first layer is selected among silicon, germanium or gallium arsenide.
In preferred embodiments of the method according to the invention the second layer can be deposited as a dispersion from a dispergent or as a dissolved material from solution or alternatively deposited in a melt-application process.
It is according to the method of the invention advantageous to select the conducting polymer in the second layer as a doped conjugated polymer and preferably select the conjugated polymer from among poly(3,4-dioxyethylene thiophene) (PEDOT), a copolymer which includes the monomer, 3,4-dioxyethylene thiophene, substituted poly(thiophenes), substituted poly(pyrroles), substituted poly(anilines) or copolymers thereof, whereas the dopant for the conjugated polymer preferably is poly(4-styrene sulphonate) (PSS).
In a preferred embodiment of the method according to the invention the doped conjugated polymer is poly(3,4-ethylenedioxythiophene) (PEDOT) doped with poly(4-styrene sulphonate) (PSS).
It is according to the invention advantageous to select the semiconducting organic material in the third layer from among conjugated polymers, or crystalline, polycrystalline, microcrystalline and amorphous organic compounds, and in case the conjugated polymer is selected, it is preferred that this is selected from among poly(2-methoxy, 5-(2′-ethylhexyloxy)-1,4-phenylene vinylene) (MEH-PPV) or poly(3-hexylthiophene) (P3HT).
Finally it is according to the invention advantageous to selecti the metal of the fourth layer from among metals which have a lower work function than that of the anode and to particularly select the metal of the fourth layer as the same as the metal selected for the first layer, but aluminium could in any case particularly be selected as the metal of the fourth layer.
The method according to the invention is used for manufacturing the electrode arrangement in an organic thin-film diode or for manufacturing electrode arrangements in a transistor structure, especially in an organic thin-film transistor a hybrid thin-film transistor.
The invention shall now be described in more detail with reference to the accompanying drawings as well as an appended example of polymer-based diodes with high rectification ratio manufactured according to the method described in the present invention.
The present invention can be used to realize electrode arrangements for organic semiconductor components in thin-film electronics. In the anode a conducting polymer is used in the form of a conjugated polymer to which has been added a suitable dopant.
In each case the embodiments of
According to the present invention anodes formed as double layers with metal, or alternatively a semiconductor or a semiconductor and a metal in combination, under a layer of a conducting polymer in the form of PEDOT-PSS improves the conductivity. The metal and the semiconductor in the anode may be Cu or Al which both possess a low work function, but in combination with PEDOT the anode appears with essentially the high work function of PEDOT. At the same time the combination of metal and PEDOT improves the conductivity of the anode. The PEDOT-PSS layer modifies the injection properties of the anode metal which has a low work function value, providing a problem-free hole injection. If the anode were made from metal only, the current flow would be limited by the contact, but the use of PEDOT-PSS ensures that the current flow now is be bulk-limited. By using a metal/PEDOT-PSS-anode it is, as shown in
Below follows examples of diodes made by the method according to the present invention and the associated current/voltage characteristics that have been achieved, and associated figures.
A large effort has been undertaken towards fabrication of electronic devices using polymers. Most of these are directed towards field-effect transistors and diodes, in imitation of silicon electronics. Among the diodes, both light emitting diodes and light detecting diodes constitute the major fraction of the studies; in both of these a transparent electrode is suitable. However, a high rectification organic diode is quite important for a broad spectrum of electronic applications. In order to fabricate diodes based on semiconducting polymers with high rectification, one needs materials that allow efficient charge injection trough the polymer under forward bias, and much less so under reverse bias. Normally this is achieved using materials that match in energy position, or make low potential barriers, to the HOMO (Highest Occupied Molecular Orbital) and LUMO (Lowest Unoccupied Molecular Orbital) levels of the polymer. In the reverse bias both barriers for electrons and holes must be high enough to keep the current low, having thus as a result a high rectification ratio. But it is not just the energy levels that matter. The interface properties and the quality of the polymer film formed onto a given metal can define the diode properties; often polymer film spin-coated onto inert materials such as gold presents pin holes that are not acceptable if one needs to evaporate an upper electrode on top of the polymer film in a sandwich geometry. The conducting/semiconducting polymer interface tends to have good adhesion. The oxidized conducting polymer poly(3,4-ethylenedioxythiophene) doped with poly(4-styrene sulphonate) (PEDOT-PSS) was found to have the high work function value 5.2 eV which allows efficient hole injection in LEDs or collectors in photodiodes. However, the higher resistance of PEDOT-PSS compared with ordinary metals may compromise the diode performance in thin patterned lines, due to voltage drop under high currents. To handle this problem, a metal layer under the polymer is used. Any metal can be used as the underlying layer as it is not necessary to match the work function of the metal (φm) with the work function of PEDOT (φPEDOT). Since noble metals like gold and platinum which is commonly used in organic light-emitting diodes, are known to comport detrimental effects when used in conjunction with PEDOT, the preferred metals will be base metals with high conductivity.—The expression “base metals” as used herein, as opposed to noble metals, should be understood as metals with electrochemical potential less than 1 volt.—Diodes made with several metals (Al (4.2 eV), Ag (4.3 eV), Cu (4.5 eV)) were tested. In all cases the current flow of holes which was contact-limited, changed to bulk-limited when a PEDOT-PSS layer was used between the anode metal and the semiconducting polymer MEH-PPV (poly(2-methoxy, 5-(2′-ethyl-hexyloxy)-1,4-phenylene vinylene)). In order to study the electrical properties of diodes with different active areas copper was chosen as the underlying layer, particularly due to its good stability and etching properties. The Cu/PEDOT-PSS interface was demonstrated to be ohmic with a contact resistance rc≈7 Ω/□. The ohmic behaviour of Cu/PEDOT-PSS interface is an important asset for its use as an electrode in diodes. The contact resistance of Cu/PEDOT-PSS interface was measured using planar geometry to provide a copper surface similar to that used for the diodes.
The diodes were constructed in sandwich geometry using Cu/PEDOT-PSS as the anode and Al as the cathode (φ=4.2 eV). They were mounted onto a glass or Si with 2 μm thick oxide substrate, as shown in
The I-V characteristics of two similar diodes made using MEH-PPV polymer is presented in
The Cu/PEDOT-PSS/MEH-PPV/Al diodes with 100 μm2 of active area presented a similar shape of the forward current-voltage characteristics, as can be seen in the insert graph in FIG. 5. In order to compare the I-V characteristics of both diodes, the current densities are plotted in
However, for a diode of this size the current level is quite low, around the noise level as can be seen in the insert graph in FIG. 5. The I-V characteristics for the current densities of both the diode with 1 gm2 active area and the one of 8 mm2 active area are plotted. The function J(V) for the smaller diode is plotted up to twenty volts. It can be seen that the behaviour and shape do not scale very well with the larger diode. With these small diodes, the area extension is only ten times the thickness of the layers, and fringe fields are expected to start becoming important; even more important may be the existing irregularities causing any geometrical estimates to err.
The electrical transport properties of conjugated polymers and polymer/metals junctions have been studied for quite some time. The first attempt in modelling the PPV based diodes was based on the Fowler-Nordheim model describing the tunnelling process in the diode. It was possible to obtain the approximate values for barrier heights and for the polymer energy levels. A number of models have since then been presented, taking in account more parameters for detailing the interface properties. It is proposed that when the current is contact-limited the effect of Coulomb trapping of carriers at the interface can be determined by the image force. This trapping results in an increase of the energy barrier height, decreasing the injection flow. It was concluded that the presence of an insulating material free of traps could increase the charge injection. In the case of PEDOT-PSS it was shown that during the deposition of this material by spin-coating, a segregation of PEDOT and PSS takes place. PSS is an insulating material and it was found to form a thin layer all over the PEDOT surface film. This thin layer cannot trap charges from the electrode which may account for the improvement in the carrier injection from PEDOT. The bulk-limited current of MEH-PPV has been studied and reported by several research groups. It was found that at high fields MEH-PPV presents a spatial charge limitation of the current, and also that mobility is dependent on the applied electric field. In the present case the behaviour is similar, as the current does not depend on V2 precisely because of the field-dependent mobility. This was proposed in a recent study by Malliaras et al., PRB, Vol 58, R13411 (1998). The use of a model developed by P. N. Murgatroyd (J.Phys. D. Vol. 3, 151 (1970)) combines spatial charge limitation dependence with the non-constant mobility in the same equation. From these models one can evaluate the data obtained herein by plotting the high field current in the function format JL3 versus (VL), where J is the current density, L the polymer thickness and V the applied voltage minus the built-in voltage of the diodes. For the present invention this enabled a data fit and gave similar values for the polymer parameters μ0 and E0. i.e. the zero field mobility and the characteristic field respectively.
In summary, the present invention provides a high rectification ratio polymer diode using two low work function metals, where the anode was modified by the introduction of a conducting polymer layer, PEDOT doped with PSS. With this surface modification it was possible to progress from a low injection contact-limited current to a high injection bulk-limited current. The PEDOT/PSS segregation might add to the charge injection by avoiding Coulomb trapping at the interface due to the force image effects. The possibility of making these diodes patterned on micrometer scale has been shown. This offers the prospect of fabricating such diodes for microelectronics with active devices such as switching diodes and switching transistors, but also in electrically addressable high-density thin-film memories in e.g. a passive matrix.
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|U.S. Classification||438/22, 257/40|
|International Classification||H01L51/30, H01L51/10, H01L21/336, H01L29/786, H01L51/00, H01L29/861, H01L51/40, H01L51/05, H01L21/28, H01L21/00|
|Cooperative Classification||Y02E10/549, H01L51/0036, H01L51/424, H01L51/0037, H01L51/0038|
|Feb 6, 2001||AS||Assignment|
Owner name: THIN FILM ELECTRONICS ASA, NORWAY
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Effective date: 20090208